Atomic Ni directional-substitution on ZnIn_(2)S_(4) nanosheet to achieve the equilibrium of elevated redox capacity and efficient carrier-kinetics performance in photocatalysis  

作　　者：Haibin Huang Guiyang Yu Xingze Zhao Boce Cui Jinshi Yu Chenyang Zhao Heyuan Liu Xiyou Li 

机构地区：[1]School of Materials Science and Engineering,China University of Petroleum(East China),Qingdao 266580,Shandong,China [2]Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science(MOE),College of Chemistry and Molecular Engineering,Qingdao University of Science and Technology,Qingdao 266042,Shandong,China [3]College of New Energy,China University of Petroleum(East China),Qingdao 266580,Shandong,China

出　　处：《Journal of Energy Chemistry》2024年第1期272-281,I0007,共11页能源化学（英文版）

基　　金：the National Natural Science Foundation of China (22209091);the Natural Science Foundation of Shandong Province (ZR2020QB057);the Key Program of National Natural Science Foundation of China (22133006);the Yankuang Group 2019 Science and Technology Program (YKKJ2019AJ05JG-R60)。

摘　　要：It is a challenge to coordinate carrier-kinetics performance and the redox capacity of photogenerated charges synchronously at the atomic level for boosting photocatalytic activity.Herein,the atomic Ni was introduced into the lattice of hexagonal ZnIn_(2)S_(4) nanosheets(Ni/ZnIn_(2)S_(4))via directionalsubstituting Zn atom with the facile hydrothermal method.The electronic structure calculations indicate that the introduction of Ni atom effectively extracts more electrons and acts as active site for subsequent reduction reaction.Besides the optimized light absorption range,the elevation of Efand ECBendows Ni/ZnIn_(2)S_(4) photocatalyst with the increased electron concentration and the enhanced reduction ability for surface reaction.Moreover,ultrafast transient absorption spectroscopy,as well as a series of electrochemical tests,demonstrates that Ni/ZnIn_(2)S_(4) possesses 2.15 times longer lifetime of the excited charge carriers and an order of magnitude increase for carrier mobility and separation efficiency compared with pristine ZnIn_(2)S_(4).These efficient kinetics performances of charge carriers and enhanced redox capacity synergistically boost photocatalytic activity,in which a 3-times higher conversion efficiency of nitrobenzene reduction was achieved upon Ni/ZnIn_(2)S_(4).Our study not only provides in-depth insights into the effect of atomic directional-substitution on the kinetic behavior of photogenerated charges,but also opens an avenue to the synchronous optimization of redox capacity and carrier-kinetics performance for efficient solar energy conversion.

关 键 词：ZnIn_(2)S_(4) SUBSTITUTION Carrier kinetics Redox capacity PHOTOCATALYSIS 

分 类 号：O643.36[理学—物理化学] O644.1[理学—化学] TB383.1[一般工业技术—材料科学与工程]